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Title: Diffusive dynamics during the high-to-low density transition in amorphous ice

Water exists in high- and low-density amorphous ice forms (HDA and LDA), which could correspond to the glassy states of high- (HDL) and low-density liquid (LDL) in the metastable part of the phase diagram. However, the nature of both the glass transition and the high-to-low-density transition are debated and new experimental evidence is needed. Here we combine wide-angle X-ray scattering (WAXS) with X-ray photon-correlation spectroscopy (XPCS) in the small-angle X-ray scattering (SAXS) geometry to probe both the structural and dynamical properties during the high-to-low-density transition in amorphous ice at 1 bar. By analyzing the structure factor and the radial distribution function, the coexistence of two structurally distinct domains is observed at T = 125 K. XPCS probes the dynamics in momentum space, which in the SAXS geometry reflects structural relaxation on the nanometer length scale. The dynamics of HDA are characterized by a slow component with a large time constant, arising from viscoelastic relaxation and stress release from nanometer-sized heterogeneities. Above 110 K a faster, strongly temperature-dependent component appears, with momentum transfer dependence pointing toward nanoscale diffusion. This dynamical component slows down after transition into the low-density form at 130 K, but remains diffusive. In conclusion, the diffusive character ofmore » both the high- and low-density forms is discussed among different interpretations and the results are most consistent with the hypothesis of a liquid–liquid transition in the ultraviscous regime.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [2] ;  [5] ;  [2] ;  [2] ;  [1] ;  [2] ;  [2] ;  [4] ;  [6] ;  [6] ;  [7] ; ORCiD logo [6] ;  [3] ;  [2] ;  [2]
  1. Stockholm Univ., Stockholm (Sweden); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Stockholm Univ., Stockholm (Sweden)
  3. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
  4. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  5. KTH Royal Institute of Technology, Stockholm (Sweden)
  6. Univ. of Innsbruck, Innsbruck (Austria)
  7. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515; 667205; 2013-3737-VR; P2ZHP2 148666; I1392; EXC1074; AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 31; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; liquid–liquid transition; glass transition; amorphous ice; X-ray photon-correlation spectroscopy; supercooled water
OSTI Identifier:
1390292
Alternate Identifier(s):
OSTI ID: 1393142

Perakis, Fivos, Amann-Winkel, Katrin, Lehmkuhler, Felix, Sprung, Michael, Mariedahl, Daniel, Sellberg, Jonas A., Pathak, Harshad, Spah, Alexander, Cavalca, Filippo, Schlesinger, Daniel, Ricci, Alessandro, Jain, Avni, Massani, Bernhard, Aubree, Flora, Benmore, Chris J., Loerting, Thomas, Grubel, Gerhard, Pettersson, Lars G. M., and Nilsson, Anders. Diffusive dynamics during the high-to-low density transition in amorphous ice. United States: N. p., Web. doi:10.1073/pnas.1705303114.
Perakis, Fivos, Amann-Winkel, Katrin, Lehmkuhler, Felix, Sprung, Michael, Mariedahl, Daniel, Sellberg, Jonas A., Pathak, Harshad, Spah, Alexander, Cavalca, Filippo, Schlesinger, Daniel, Ricci, Alessandro, Jain, Avni, Massani, Bernhard, Aubree, Flora, Benmore, Chris J., Loerting, Thomas, Grubel, Gerhard, Pettersson, Lars G. M., & Nilsson, Anders. Diffusive dynamics during the high-to-low density transition in amorphous ice. United States. doi:10.1073/pnas.1705303114.
Perakis, Fivos, Amann-Winkel, Katrin, Lehmkuhler, Felix, Sprung, Michael, Mariedahl, Daniel, Sellberg, Jonas A., Pathak, Harshad, Spah, Alexander, Cavalca, Filippo, Schlesinger, Daniel, Ricci, Alessandro, Jain, Avni, Massani, Bernhard, Aubree, Flora, Benmore, Chris J., Loerting, Thomas, Grubel, Gerhard, Pettersson, Lars G. M., and Nilsson, Anders. 2017. "Diffusive dynamics during the high-to-low density transition in amorphous ice". United States. doi:10.1073/pnas.1705303114. https://www.osti.gov/servlets/purl/1390292.
@article{osti_1390292,
title = {Diffusive dynamics during the high-to-low density transition in amorphous ice},
author = {Perakis, Fivos and Amann-Winkel, Katrin and Lehmkuhler, Felix and Sprung, Michael and Mariedahl, Daniel and Sellberg, Jonas A. and Pathak, Harshad and Spah, Alexander and Cavalca, Filippo and Schlesinger, Daniel and Ricci, Alessandro and Jain, Avni and Massani, Bernhard and Aubree, Flora and Benmore, Chris J. and Loerting, Thomas and Grubel, Gerhard and Pettersson, Lars G. M. and Nilsson, Anders},
abstractNote = {Water exists in high- and low-density amorphous ice forms (HDA and LDA), which could correspond to the glassy states of high- (HDL) and low-density liquid (LDL) in the metastable part of the phase diagram. However, the nature of both the glass transition and the high-to-low-density transition are debated and new experimental evidence is needed. Here we combine wide-angle X-ray scattering (WAXS) with X-ray photon-correlation spectroscopy (XPCS) in the small-angle X-ray scattering (SAXS) geometry to probe both the structural and dynamical properties during the high-to-low-density transition in amorphous ice at 1 bar. By analyzing the structure factor and the radial distribution function, the coexistence of two structurally distinct domains is observed at T = 125 K. XPCS probes the dynamics in momentum space, which in the SAXS geometry reflects structural relaxation on the nanometer length scale. The dynamics of HDA are characterized by a slow component with a large time constant, arising from viscoelastic relaxation and stress release from nanometer-sized heterogeneities. Above 110 K a faster, strongly temperature-dependent component appears, with momentum transfer dependence pointing toward nanoscale diffusion. This dynamical component slows down after transition into the low-density form at 130 K, but remains diffusive. In conclusion, the diffusive character of both the high- and low-density forms is discussed among different interpretations and the results are most consistent with the hypothesis of a liquid–liquid transition in the ultraviscous regime.},
doi = {10.1073/pnas.1705303114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 31,
volume = 114,
place = {United States},
year = {2017},
month = {6}
}